We demonstrate controlled charge trapping and release,a ccompanied by multiple color changes in am etalloorganic bilayer.T he dual functionality of the metallo-organic materials provides fundamental insight into the metal-mediated electron transport pathways. The electrochemical processes are visualizedb yd istinct, four color-to-color transitions: red, transparent, orange,and brown. The bilayer is composed of two elements:1 )a nanoscale gate consisting of al ayer of well-defined polypyridyl ruthenium complexes bound to af lexible transparent electrode,a nd 2) ac harge storage layer consisting of isostructural iron complexes attached to the surface of the gate.T his gate mediates or blocks electron transport in response to an applied voltage.The charge storage and release depend on the oxidation state of the layer of ruthenium complexes (= gate). Combining electrochemistry with optical data revealed mechanistic information:the brown coloration of the bilayer directly relates to the formation of intermediate ruthenium species,p roviding evidence for catalytic positive charge release mediated through the gate.[*] Y. Hamo, Dr.M.L ahav,P rof. M. E. van der Boom